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SmSe is Wurtzite structured and crystallizes in the hexagonal P6_3mc space group. The structure is three-dimensional. Sm2+ is bonded to four equivalent Se2- atoms to form corner-sharing SmSe4 tetrahedra. All Sm–Se bond lengths are 2.84 Å. Se2- is bonded to four equivalent Sm2+ atoms to form corner-sharing SeSm4 tetrahedra.
SmSe is Halite, Rock Salt structured and crystallizes in the cubic Fm-3m space group. The structure is three-dimensional. Sm2+ is bonded to six equivalent Se2- atoms to form a mixture of edge and corner-sharing SmSe6 octahedra. The corner-sharing octahedral tilt angles are 0°. All Sm–Se bond lengths are 2.95 Å. Se2- is bonded to six equivalent Sm2+ atoms to form a mixture of edge and corner-sharing SeSm6 octahedra. The corner-sharing octahedral tilt angles are 0°.